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arXiv:quant-ph/0507087 · Physical Review Letters

Efficient and Long-Lived Field-Free Orientation of Molecules by a Single Hybrid Short Pulse

D. Daems, S. Guérin, Dominique Sugny, Hans Rudolf Jauslin

Published Apr 20, 2005• 92 citations
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Abstract

We show that a combination of a half-cycle pulse and a short nonresonant laser pulse produces a strongly enhanced postpulse orientation. Robust transients that display both efficient and long-lived orientation are obtained. The mechanism is analyzed in terms of optimal oriented target states in finite Hilbert subspaces and shows that hybrid pulses can prove useful for other control issues.

DOI
10.1103/physrevlett.94.153003

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Efficient and long-lived field-free molecular orientation is achieved using only two kicks appropriately delayed in time. The understanding of the mechanism rests upon a molecular target state providing the best efficiency versus persistence compromise. An optimal control scheme is referred to for fixing the free parameters (amplitudes and the time delay between them). The limited number of kicks, the robustness and the transposability to different molecular systems advocate in favor of the process, when considering its experimental feasibility.
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We explore the possibility of forming a oriented polar molecule directly from a pair of colliding atoms. The process comprises the photoassociation and vibrational stabilization along with the molecular orientation. These processes are driven by a single time-dependent, linearly polarized control field and proceeds entirely within the electronic ground state, leveraging the presence of a permanent dipole moment. The control field is found by means of an optimal quantum control algorithm with a single target observable given by the restriction of the orientation operator on a subset of bound levels. We consider a rovibrational model system for the collision of O + H atoms and solve directly the time-dependent Schrodinger equation. We show that the optimized field is capable of enhancing the molecular orientation already induced by the photoassociation and vibrational stabilization thus yielding oriented polar molecules that can be useful for many applications.